1. Swedish University of Agricultural Sceinces Updated heavy metal budgets and critical loads Lage Bringmark & Lars Lundin

2. Swedish University of Agricultural Sceinces Trace metal budgets and critical loads – update and discussion Priority metals: Pb, Cd, Hg Authors: Lage Bringmark (SE), Lars Lundin (SE), Helga Dieffenbach-Fries (DE), Buchard Beudert (DE), Maria Theresia Grabner (AT), Thomas Dirnböck, (AT), Tuija Ruoho-Airola (FI), Iraida Lyulka (LV), Milan Vana (CZ), Pavel Kram (CZ) and Algirdas Augustaitis (LT).

3. Swedish University of Agricultural Sceinces Sites and Flows of lead (Pb) in bulk deposition (BD), throughfall (TF) and steam water runoff (RW) at IMCP IM sites for one or more years during 1996-2008 (mg.m -2.yr -1 ) BDTFLFRW SE16, Gammtratten0.770.710.460.10 SE15, Kindla1.221.060.920.20 SE14, Aneboda0.761.081.230.29 FI03, Hietajärvi0.570.530.04 FI01, Valkea-Kotonen0.650.12 LV02, Zoseni1.010.910.06 LV01, Rucava1.901.760.11 LT01, Aukstatija0.860.09 LT03, Zematija1.940.24 CZ02, Lysina0.620.670.88 CZ01, Anenske Povodi2.831.340.07 DE01, Forellenbach1.261.691.441.42 AT01, Zöbelboden, beech0.930.860.730.31 AT01, Zöbelboden, spruce0.931.690.620.31

4. Swedish University of Agricultural Sceinces Lead balances for the Finnish FI03 catchment and the three Swedish catchments SE14, SE15, and SE16 with throughfall, TF, litterfall, LF, and runoff, RW included. TF+LF is also included

5. Input Approximate estimate of total deposition, TD TD = TF + LF Swedish University of Agricultural Sceinces

6. Mercury balances for the four Swedish catchments SE 04, SE 14, SE 15 and SE 16 showing throughfall, TF, litterfall, LF and runoff, RW.

7. Swedish University of Agricultural Sceinces Metal content in the humus layer during 1985-2010 in the IM site SE14

8. Swedish University of Agricultural Sceinces Bulk deposition (µg.m -2 ) at SE04 Gårdsjön YearCdPb 1996481727 1997531810 1998341294 1999541887 2000551653 200129921 200235949 200336857 220436988 200535898 200641889 200732787 200824508

9. Swedish University of Agricultural Sceinces Stream concentrations at SE14 Aneboda, Pb µg.L -1

10. Swedish University of Agricultural Sceinces Hovmand et al, 2008, Env. Pollution 155: 537-541 Bulk deposition 50 yr – Pb (Pacyna) 430 mg.m -2 (TF+LF approx.1300 mg.m -2 ) Bulk deposition 50 yr – Cd (Pacyna) 6.7 mg.m -2 (TF+LF approx. 27 mg.m -2 ) Bulk deposition 50 yr – Hg (Bringmark) ≈ 2.0 mg.m -2 (TF+LF approx.16 mg.m -2 ) ------------------ South Swedish soil stores 1995 1996, mg.m -2 AnebodaGårdsjön Pbhumus layer 680 690 humus layer plus 20 cm28003400 Cd humus layer 3.82.4 humus layer plus 20 cm 19 Hghumus layer2.32.2 humus layer plus 20 cm9.19.0

11. Swedish University of Agricultural Sceinces Critical loads Cd Pb Hg On request from WGE, Europe-wide task of calculating and mapping critical loads and exceedances. Call for data in 2004. EMEP grid cells. Deposition by EMEP modelling. Exceedance of 5th percentile of critical load in each grid cell. Results on soil ecotoxicological endpoints; exceedance 0.4% of land area for Cd exceedance 12% of land area for Pb exceedance 54% of land area for Hg based on Hg in fish, 3 countries, 97-100% of area CCE 2010. Critical loads of Heavy Metals and their Exceedances. CCE Status Report 2010, 91-100.

12. Swedish University of Agricultural Sceinces Starting point for critical load calculation – critical limit Five possible endpoints for critical load calculation – critical limit Five possible endpoints in the manual 1)drinking water – human health 2) terrestrial food quality – human health 3) terrestrial eco-toxicological effects (mainly soils) 4)aquatic food quality – human health (Hg in fish) 1-3, relation to metal concentration in soil solution 4, empiric relation to concentration in rainfall (Hg)

13. Swedish University of Agricultural Sceinces Critical limit for Hg, most important point and most weak South Swedish concentrations of Hg in humus layer taken as critical limit at 0.5 µg.g -1 organic. Experimental effect conc ≈ 2 µg.g -1, field observations of metal effects not independent of Pb Two recent papers on critical effect concentrations for Hg: Tipping et al 2010. Environmental Pollution 158:2465-2471 crit. limit 3.3 µg.g -1 Åkerblom et al. 2010. Ecotoxicology and Environ. Safety 73: 924-931 EC5% 0.8 µg.g -1

14. Swedish University of Agricultural Sceinces 52 biological endpoints (plants, invertebrates and mainly microbes) collected from literature on experimental Hg additions. Harmonization of all experiments by recalculation to free Hg 2+ ion (WHAM). Critical limit derived from 5th percentile of species sensitivity distributions. Result: 0.13 µg.g -1 (soil) or 3.3 µg.g -1 (organic mtrl) Tipping et al., 2010 Critical limit estimations

15. Swedish University of Agricultural Sceinces Focus on most sensitive soil layer. Upper part of humus layer – high biological activity, site of metal accumulation. Lower part less sensitive, uppermost litter layer less sensitive. Effect concentration, EC5 at 0.8 g.g -1 (organic mtrl.) Correlation: Microbial activity – metal sensitivity. Northern sites more sensitive than southern ones. Åkerblom et al., 2010 Critical limit estimations in Sweden

16. Swedish University of Agricultural Sceinces Soil effect concentrations for mercury Current - 0.5 µg.g -1 (organic mtrl) Tipping - 3.3 µg.g -1 (organic mtrl) Åkerblom- 0.8 µg.g -1 (organic mtrl) Existing Hg concentrations in forest humus layers: North Sweden, general 0.2 µg.g -1, chloralcali industry 0.9 µg.g -1 South Sweden, general 0.35 µg.g -1 Czech Republic, general 0.7 µg.g -1, DE01 0.4-0.8 µg.g -1 ; (Steinkreutz, 0.16 µg.g -1 )

17. Swedish University of Agricultural Sceinces Hg accumulation is still ongoing Thank You for attention